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Integrative catalytic pairs for efficient multi-intermediate catalysis

Nature Nanotechnology volume 19, pages 1442–1451 (2024)Cite this article

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Abstract

Single-atom catalysts (SACs) have attracted considerable research interest owing to their combined merits of homogeneous and heterogeneous catalysts. However, the uniform and isolated active sites of SACs fall short in catalysing complex chemical processes that simultaneously involve multiple intermediates. In this Review, we highlight an emerging class of catalysts with adjacent binary active centres, which is called integrative catalytic pairs (ICPs), showing not only atomic-scale site-to-site electronic interactions but also synergistic catalytic effects. Compared with SACs or their derivative dual-atom catalysts (DACs), multi-interactive intermediates on ICPs can overcome kinetic barriers, adjust reaction pathways and break the universal linear scaling relations as the smallest active units. Starting from this active-site design principle, each single active atom can be considered as a brick to further build integrative catalytic clusters (ICCs) with desirable configurations, towards trimer or even larger multi-atom units depending on the requirement of a given reaction.

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Fig. 1: Progress in developing atomically precise catalysts.
Fig. 2: Structural characterization of Ir1–P1/ICP and its principle to lower the kinetic barrier of HOR.
Fig. 3: Tandem mechanism of C–C bond formation via a formyl-bicarbonate coupling pathway on Sn1–O1/ICP.
Fig. 4: Comparison of the limitation from linear scaling relationships for SAC, DAC and ICP systems.

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Acknowledgements

This work was financially supported by the City University of Hong Kong startup fund (no. 9020003) and ITF−RTH−Global STEM Professorship (no. 9446006). H.B.Y. acknowledges support from the National Natural Science Foundation of China under grant number 22075195. C.S. gratefully thanks financial support from National Key Research and Development Program of China (number 2021YFA1600800633), National Natural Science Foundation of China (number 22372102) and Shenzhen Science and Technology Program (number RCJC20200714114434086).

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  1. These authors contributed equally: Qilun Wang, Yaqi Cheng.

Authors and Affiliations

  1. Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong SAR, China

    Qilun Wang, Yaqi Cheng & Bin Liu

  2. International Collaboration Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen, China

    Qilun Wang & Chenliang Su

  3. School of Materials Science and Engineering, Suzhou University of Science and Technology, Suzhou, China

    Hong Bin Yang

  4. Department of Chemistry, Hong Kong Institute of Clean Energy (HKICE) and Center of Super-Diamond and Advanced Films (COSDAF), City University of Hong Kong, Hong Kong SAR, China

    Bin Liu

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Wang, Q., Cheng, Y., Yang, H.B. et al. Integrative catalytic pairs for efficient multi-intermediate catalysis. Nat. Nanotechnol. 19, 1442–1451 (2024). https://doi.org/10.1038/s41565-024-01716-z

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